Biobased nanocomposite films for food packaging with high mechanical strength and good oxygen-barrier performance were developed using a hot-water wood extract (HWE). In this work, a facile approach to produce HWE/montmorillonite (MMT) based nanocomposite films with excellent physical properties is described. The focus of this study was to determine the effects of the MMT content on the structure and mechanical properties of nanocomposites and the effects of carboxymethyl cellulose (CMC) on the physical properties of the HWE-MMT films. The experimental results suggested that the intercalation of HWE and CMC in montmorillonite could produce compact, robust films with a nacre-like structure and multifunctional characteristics. This results of this study showed that the mechanical properties of the film designated FCMC0.05 (91.5 MPa) were dramatically enhanced because the proportion of HWE, MMT and CMC was 1:1.5:0.05. In addition, the optimized films exhibited an oxygen permeability below 2.0 cm3 μm/day·m2·kPa, as well as good thermal stability due to the small amount of CMC. These results provide a comprehensive understanding for further development of high-performance nanocomposites which are based on natural polymers (HWE) and assembled layered clays (MMT). These films offer great potential in the field of sustainable packaging.